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Mosaic crystals, with their high integrated reflectivities, are widely employed in spectrometers used to diagnose high energy density systems. X-ray Thomson scattering (XRTS) has emerged as a powerful diagnostic tool of these systems, providing in principle direct access to important properties such as the temperature via detailed balance. However, the measured XRTS spectrum is broadened by the spectrometer instrument function (IF), and without careful consideration of the IF one risks misdiagnosing system conditions. Here, we consider in detail the IF of 40 and 100 μ m mosaic Highly Annealed Pyrolytic Graphite crystals, and how the broadening varies across the spectrometer in an energy range of 6.7–8.6 keV. Notably, we find a strong asymmetry in the shape of the IF toward higher energies. As an example, we consider the effect of the asymmetry in the IF on the temperature inferred via XRTS for simulated 80 eV CH plasmas and find that the temperature can be overestimated if an approximate symmetric IF is used. We, therefore, expect a detailed consideration of the full IF will have an important impact on system properties inferred via XRTS in both forward modeling and model-free approaches. [ABSTRACT FROM AUTHOR]

We investigated the effect of the NaCl concentration (0.3–2M) on the structure and dynamics of hen egg yolk at room temperature and during thermal gelation at temperatures in the range of 66–90 °C utilizing low-dose x-ray photon correlation spectroscopy in ultra-small angle x-ray scattering geometry. With an increase in the salt concentration, we observe progressive structural and dynamic changes at room temperature, indicating the disruption of yolk components such as yolk-granules and yolk-plasma proteins. Temperature- and salt-dependent structural and dynamic investigations suggest a delay in the gel formation and aggregation of yolk low-density lipoproteins with increasing ionic strength. However, the time–temperature superposition relationship observed in all samples suggests an identical mechanism underlying protein aggregation–gelation with a temperature-dependent reaction rate. The sol–gel transition time extracted from kinetic and dynamic information follows Arrhenius's behavior, and the activation energy (460 kJ/mol) is found to be independent of the salt concentration. [ABSTRACT FROM AUTHOR]

The unfolding dynamics of ubiquitin were studied using a combination of x-ray solution scattering (XSS) and molecular dynamics (MD) simulations. The kinetic analysis of the XSS ubiquitin signals showed that the protein unfolds through a two-state process, independent of the presence of destabilizing salts. In order to characterize the ensemble of unfolded states in atomic detail, the experimental XSS results were used as a constraint in the MD simulations through the incorporation of x-ray scattering derived potential to drive the folded ubiquitin structure toward sampling unfolded states consistent with the XSS signals. We detail how biased MD simulations provide insight into unfolded states that are otherwise difficult to resolve and underscore how experimental XSS data can be combined with MD to efficiently sample structures away from the native state. Our results indicate that ubiquitin samples unfolded in states with a high degree of loss in secondary structure yet without a collapse to a molten globule or fully solvated extended chain. Finally, we propose how using biased-MD can significantly decrease the computational time and resources required to sample experimentally relevant nonequilibrium states. [ABSTRACT FROM AUTHOR]

We investigated the structure of ice under nanoporous confinement in periodic mesoporous organosilicas (PMOs) with different organic functionalities and pore diameters between 3.4 and 4.9 nm. X-ray scattering measurements of the system were performed at temperatures between 290 and 150 K. We report the emergence of ice I with both hexagonal and cubic characteristics in different porous materials, as well as an alteration of the lattice parameters when compared to bulk ice. This effect is dependent on the pore diameter and the surface chemistry of the respective PMO. Investigations regarding the orientation of hexagonal ice crystals relative to the pore wall using x-ray cross correlation analysis reveal one or more discrete preferred orientation in most of the samples. For a pore diameter of around 3.8 nm, stronger correlation peaks are present in more hydrophilically functionalized pores and seem to be connected to stronger shifts in the lattice parameters. [ABSTRACT FROM AUTHOR]

Compared with batch and vapor diffusion methods, counter diffusion can generate larger and higher-quality protein crystals yielding improved diffraction data and higher-resolution structures. Typically, counter-diffusion experiments are conducted in elongated chambers, such as glass capillaries, and the crystals are either directly measured in the capillary or extracted and mounted at the X-ray beamline. Despite the advantages of counter-diffusion protein crystallization, there are few fixed-target devices that utilize counter diffusion for crystallization. In this article, different designs of user-friendly counter-diffusion chambers are presented which can be used to grow large protein crystals in a 2D polymer microfluidic fixed-target chip. Methods for rapid chip fabrication using commercially available thin-film materials such as Mylar, propyl-ene and Kapton are also detailed. Rules of thumb are provided to tune the nucleation and crystal growth to meet users' needs while minimizing sample consumption. These designs provide a reliable approach to forming large crystals and maintaining their hydration for weeks and even months. This allows ample time to grow, select and preserve the best crystal batches before X-ray beam time. Importantly, the fixed-target microfluidic chip has a low background scatter and can be directly used at beamlines without any crystal handling, enabling crystal quality to be preserved. The approach is demonstrated with serial diffraction of photoactive yellow protein, yielding 1.32 Å resolution at room temperature. Fabrication of this standard microfluidic chip with commercially available thin films greatly simplifies fabrication and provides enhanced stability under vacuum. These advances will further broaden microfluidic fixed-target utilization by crystallographers.

Here, we investigate the hypothesis that despite the existence of at least two high-density amorphous ices, only one high-density liquid state exists in water. We prepared a very-high-density amorphous ice (VHDA) sample and rapidly increased its temperature to around 205 ± 10 K using laser-induced isochoric heating. This temperature falls within the so-called "no-man's land" well above the glass-liquid transition, wherein the IR laser pulse creates a metastable liquid state. Subsequently, this high-density liquid (HDL) state of water decompresses over time, and we examined the time-dependent structural changes using short x-ray pulses from a free electron laser. We observed a liquid–liquid transition to low-density liquid water (LDL) over time scales ranging from 20 ns to 3 μs, consistent with previous experimental results using expanded high-density amorphous ice (eHDA) as the initial state. In addition, the resulting LDL derived both from VHDA and eHDA displays similar density and degree of inhomogeneity. Our observation supports the idea that regardless of the initial annealing states of the high-density amorphous ices, the same HDL and final LDL states are reached at temperatures around 205 K. [ABSTRACT FROM AUTHOR]

The temperature-induced phase and morphology changes of a thin layer sandwiched between two substrates which it partially wets are investigated using transmission electron microscopy, scanning electron microscopy, and x-ray scattering techniques. For this, SiC wafers were bonded with Si layers of various thicknesses and annealed at temperatures below and above the Si melting point. Below the melting point of Si, solid-state dewetting occurs. It starts with the heterogeneous nucleation of pits at the Si/SiC interfaces and progresses to their partial transformation into voids crossing the whole film. The further growth of voids is accompanied with an increase in the Si film thickness. Final equilibrium is shown to be impacted by Si crystallographic state evolution. Above the Si melting temperature, liquid Si drives SiC interfaces step bunching. When high steps and large terraces are formed over the two SiC surfaces, Si is shown to be trapped within quasi-closed pockets. Eventually, the interface locally closes around these Si inclusions with the creation of SiC/SiC direct contacts. The influence of both annealing temperatures and Si film thickness on all these processes is discussed. [ABSTRACT FROM AUTHOR]

There is no consensus among researchers regarding how phase transitions occur in antiferroelectric (AFE) epitaxial heterostructures, in particular, in heterostructures based on model AFE lead zirconate. The questions about the number of phase transitions in such films and by what mechanism they occur remain controversial. This paper presents a look at the phase transition scenario in two types of epitaxial heterostructures: PbZrO 3 /Ba[La–Sn]O 3 /MgO (001) thin films with thicknesses from 25 to 1000 nm and PbZrO 3 /SrRuO 3 /SrTiO 3 (001) thin film 100 nm thick using the diffuse x-ray scattering in the grazing incidence setup. We register the characteristic butterfly-shaped diffuse scattering (DS) intensity distribution in the H K pseudocubic planes, which corresponds to the anisotropic ferroelectric soft mode. No incommensurate soft mode was observed in the cuts of reciprocal space parallel to the film surface by diffuse scattering. We reproduce the shape of DS distribution at different temperatures by the model based on the dielectric stiffness and the electric polarization correlation tensor in the cubic approximation. Such modeling allows not only to characterize the DS parameters from the challengingly low signal-to-background data set, but also to extract experimentally the sensitivity of the materials with respect to inhomogeneous polarization. While the observed temperature evolution of DS is consistent with the dielectric measurements, the correlation between the DS and the phase transition sequence observed by superstructure reflections is yet to be understood better. [ABSTRACT FROM AUTHOR]

We investigated the spectrum of density fluctuations of a liquid crystal, CB7CB, in two different orientations by using high-resolution inelastic x-ray scattering. Our analysis, based on Bayesian principles, revealed that high-frequency collective excitations propagate through this mesoscale-ordered sample in a peculiar manner that lies somewhere between those observed in liquids and crystalline systems. Interestingly, when we probed longer length scales, a more pronounced solid-like response emerged. This was mainly characterized by anomalously sharp inelastic excitations and the onset of shear mode propagation. Comparison with previous x-ray diffraction results suggests a correlation between the observed behavior and the mesogen arrangement. [ABSTRACT FROM AUTHOR]

Small angle x-ray scattering (SAXS) stands out as a promising solution in semiconductor metrology. The critical issue of SAXS metrology is to solve the SAXS inverse problem. With the increasing complexity of semiconductor devices, traditional strategies will face problems such as long iteration time and multiple solutions. To address these challenges, we develop a physical symmetry enhanced method to speed up the solution of the SAXS inverse problem for complex nanostructures. We incorporate the physical symmetry into a deep learning model, and a combined loss function is proposed to determine the correct structure in each step of training, which can continuously correct errors and make the model converge faster. The results show that the proposed method achieves high accuracy in determining the critical structural parameters of the complex profile gratings. Compared to traditional strategies, our method performs better in accuracy and does not require time-consuming iterations during reconstruction. The physical symmetry enhanced method provides a feasible way for achieving real-time reconstruction of complex profile nanostructures and is expected to promote the development of SAXS metrology. [ABSTRACT FROM AUTHOR]

A combination of experimental and numerical investigations on metallic silver and platinum nanoparticles deposited on silica substrates is presented, with a focus on metal–substrate interactions. Experimentally, the nanoparticles, obtained by ultra-high vacuum atom deposition, are characterized by grazing-incidence small-angle x-ray scattering and high resolution transmission electronic microscopy to determine their structure and morphology and, in particular, their aspect ratio (height/diameter), which quantifies the metal–substrate interaction, from the as-grown to equilibrium state. Numerically, the interactions between the metal and the silica species are modeled with the Lennard-Jones (12, 6) potential, with two parameters for each metal and silica species. The geometric parameters were found in the literature, while the energetic parameters were determined from our experimental measurements of the aspect ratio. The parameters are as follows: σAg–O = 0.278 nm, σAg–Si = 0.329 nm, ɛAg–O = 75 meV, and ɛAg–Si = 13 meV for Ag–silica and σPt–O = 0.273 nm, σPt–Si = 0.324 nm, ɛPt–O = 110 meV, and ɛPt–Si = 18 meV for Pt–silica. The proposed Ag–silica potential reproduces quantitatively the unexpected experimental observation of the variation of the aspect ratio for Ag nanoparticles larger than 5 nm, which has been interpreted as a consequence of the silica roughness. The nanoparticle orientation, structure, and disorder are also considered. This metal–silica potential for Ag and Pt should be helpful for further studies on pure metals as well as their alloys. [ABSTRACT FROM AUTHOR]

Poly(ethylene oxide) (PEO)-based composite electrolytes (PCEs) are considered as promising candidates for next-generation lithium-metal batteries (LMBs) due to their high safety, easy fabrication, and good electrochemical stability. Here, we utilize operando grazing-incidence small-angle and wide-angle X-ray scattering to probe the correlation of electrochemically induced changes and the buried morphology and crystalline structure of the PCE. Results show that the two irreversible reactions, PEO-Li+ reduction and TFSI- decomposition, cause changes in the crystalline structure, array orientation, and morphology of the PCE. In addition, the reversible Li plating/stripping process alters the inner morphology, especially the PEO-LiTFSI domain radius and distance between PEO-LiTFSI domains, rather than causing crystalline structure and orientation changes. This work provides a new path to monitor a working battery in real time and to a detailed understanding of the Li+ diffusion mechanism, which is essential for developing highly transferable and interface-stable PCE-based LMBs.

In this study, we investigated the self-ordering process in Langmuir films of polydisperse iron oxide nanoparticles on a water surface, employing in situ x-ray scattering, surface pressure-area isotherm analysis, and Brewster angle microscopy. X-ray reflectometry confirmed the formation of a monolayer, while grazing incidence small-angle x-ray scattering revealed short-range lateral correlations with a characteristic length equal to the mean particle size. Remarkably, our findings indicated that at zero surface pressure, the particles organized into submicrometer clusters, merging upon compression to form a homogeneous layer. These layers were subsequently transferred to a solid substrate using the Langmuir–Schaefer technique and further characterized via scanning electron microscopy and polarized neutron reflectometry. Notably, our measurements revealed a second characteristic length in the lateral correlations, orders of magnitude longer than the mean particle diameter, with polydisperse particles forming circular clusters densely packed in a hexagonal lattice. Furthermore, our evidence suggests that the lattice constant of this mesocrystal depends on the characteristics of the particle size distribution, specifically the mean particle size and the width of the size distribution. In addition, we observed internal size separation within these clusters, where larger particles were positioned closer to the center of the cluster. Finally, polarized neutron reflectometry measurements provided valuable insights into the magnetization profile across the layer. [ABSTRACT FROM AUTHOR]

In this study, the total ion yield near-edge x-ray absorption fine structure spectra of four similar peptoid molecules, which differ in the numbers and positions of methyl groups, were investigated experimentally and theoretically. At each excitation energy, the intensity and branching ratio of each ionic product were measured. At a few resonant excitation energies, a specific dissociation of the C–CO bond at the nitrogen and oxygen K-edges and of the N–CO bond at the carbon K-edge was dominant, which correlated well with the predicted destination antibonding orbitals of the core electron excitation. These specific dissociation mechanisms of small peptoid molecules could provide insights into similar phenomena that occur in peptide molecules. [ABSTRACT FROM AUTHOR]

In the present paper, we apply a blind fitting algorithm to model two-dimensional energy-incidence angle maps of soft x-ray resonant reflectivity measured in nanoscale epitaxial multilayers of multiferroic ε-Fe2O3 grown by pulsed laser deposition. The possibility of fitting the spectral shape of the complex refraction index across the Fe L3 absorption edge without having an initial guess about the optical constants has been demonstrated. The spectral shape fitting of the real (f1) and imaginary (f2) parts of the atomic scattering factor has been carried out by using a specially designed software utilizing OpenCL fast calculations on graphical processing units. The Kramers-Kronig relations between f1 and f2 are automatically taken into account by the fitting algorithm. A reasonable agreement between blindly generated and reference scattering factor spectra derived independently from an x-ray absorption spectroscopy experiment has been demonstrated. The blind fitting has been compared with the alternative refinement routines, in which small free variations of the reference spectral shapes (or no variations at all) have been allowed. The presented approach to the resonant x-ray reflectometry modeling makes it unnecessary to acquire the optical constant spectral shapes in advance and, thus, is especially helpful when such spectra cannot be physically measured, e.g., for a buried layer of a multilayer system. [ABSTRACT FROM AUTHOR]

The ability to study chemical dynamics on ultrafast timescales has greatly advanced with the introduction of X-ray free electron lasers (XFELs) providing short pulses of intense X-rays tailored to probe atomic structure and electronic configuration. Fully exploiting the full potential of XFELs requires specialized experimental endstations along with the development of techniques and methods to successfully carry out experiments. The liquid jet endstation (LJE) at the Linac Coherent Light Source (LCLS) has been developed to study photochemistry and biochemistry in solution systems using a combination of X-ray solution scattering (XSS), X-ray absorption spectroscopy (XAS), and X-ray emission spectroscopy (XES). The pump-probe setup utilizes an optical laser to excite the sample, which is subsequently probed by a hard X-ray pulse to resolve structural and electronic dynamics at their intrinsic femtosecond timescales. The LJE ensures reliable sample delivery to the X-ray interaction point via various liquid jets, enabling rapid replenishment of thin samples with millimolar concentrations and low sample volumes at the 120 Hz repetition rate of the LCLS beam. This paper provides a detailed description of the LJE design and of the techniques it enables, with an emphasis on the diagnostics required for real-time monitoring of the liquid jet and on the spatiotemporal overlap methods used to optimize the signal. Additionally, various scientific examples are discussed, highlighting the versatility of the LJE.

DLSIA (Deep Learning for Scientific Image Analysis) is a Python-based machine learning library that empowers scientists and researchers across diverse scientific domains with a range of customizable convolutional neural network (CNN) architectures for a wide variety of tasks in image analysis to be used in downstream data processing. DLSIA features easy-to-use architectures, such as autoencoders, tunable U-Nets and parameter-lean mixed-scale dense networks (MSDNets). Additionally, this article introduces sparse mixed-scale networks (SMSNets), generated using random graphs, sparse connections and dilated convolutions connecting different length scales. For verification, several DLSIA-instantiated networks and training scripts are employed in multiple applications, including inpainting for X-ray scattering data using U-Nets and MSDNets, segmenting 3D fibers in X-ray tomographic reconstructions of concrete using an ensemble of SMSNets, and leveraging autoencoder latent spaces for data compression and clustering. As experimental data continue to grow in scale and complexity, DLSIA provides accessible CNN construction and abstracts CNN complexities, allowing scientists to tailor their machine learning approaches, accelerate discoveries, foster interdisciplinary collaboration and advance research in scientific image analysis.

We used inelastic x-ray scattering methods to measure the terahertz spectrum of density fluctuations of ethanol in both liquid and solid phases. The results of a Bayesian inference-based lineshape analysis with a multiple excitation model and the comparison with a previous similar analysis on water indicate that the different structures induced by hydrogen bonds in ethanol and water have a profound influence on the respective dynamic responses, the latter being characterized by longer living and better resolved high-frequency acoustic excitations. In addition, we compare these findings with those obtained with an alternative approach based on the exponential expansion theory and ensuring sum rules fulfillment, demonstrating that the model's choice directly impacts the number of spectral modes detected. [ABSTRACT FROM AUTHOR]

The pH-dependent change in protonation of ionizable lipids is crucial for the success of lipid-based nanoparticles as mRNA delivery systems. Despite their widespread application in vaccines, the structural changes upon acidification are not well understood. Molecular dynamics simulations support structure prediction but require an a priori knowledge of the lipid packing and protonation degree. The presetting of the protonation degree is a challenging task in the case of ionizable lipids since it depends on pH and on the local lipid environment and often lacks experimental validation. Here, we introduce a methodology of combining all-atom molecular dynamics simulations with experimental total-reflection x-ray fluorescence and scattering measurements for the ionizable lipid Dlin-MC3-DMA (MC3) in POPC monolayers. This joint approach allows us to simultaneously determine the lipid packing and the protonation degree of MC3. The consistent parameterization is expected to be useful for further predictive modeling of the action of MC3-based lipid nanoparticles. [ABSTRACT FROM AUTHOR]

The precipitation of struvite, a magnesium ammonium phosphate hexahydrate (MgNH4PO4 · 6H2O) mineral, from wastewater is a promising method for recovering phosphorous. While this process is commonly used in engineered environments, our understanding of the underlying mechanisms responsible for the formation of struvite crystals remains limited. Specifically, indirect evidence suggests the involvement of an amorphous precursor and the occurrence of multi-step processes in struvite formation, which would indicate non-classical paths of nucleation and crystallization. In this study, we use synchrotron-based in situ x-ray scattering complemented by cryogenic transmission electron microscopy to obtain new insights from the earliest stages of struvite formation. The holistic scattering data captured the structure of an entire assembly in a time-resolved manner. The structural features comprise the aqueous medium, the growing struvite crystals, and any potential heterogeneities or complex entities. By analysing the scattering data, we found that the onset of crystallization causes a perturbation in the structure of the surrounding aqueous medium. This perturbation is characterized by the occurrence and evolution of Ornstein-Zernike fluctuations on a scale of about 1 nm, suggesting a non-classical nature of the system. We interpret this phenomenon as a liquid-liquid phase separation, which gives rise to the formation of the amorphous precursor phase preceding actual crystal growth of struvite. Our microscopy results confirm that the formation of Mg-struvite includes a short-lived amorphous phase, lasting >10 s. [ABSTRACT FROM AUTHOR]

Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with promising functionalities. Mechanistic studies are still needed to uncover the design principles for SL self-assembly, but such studies have been difficult to perform due to the fast time and short length scales of NC systems. To address this challenge, we developed an apparatus to directly measure the evolving phases in situ and in real time of an electrostatically stabilized Au NC solution before, during, and after it is quenched to form SLs using small-angle X-ray scattering. By developing a quantitative model, we fit the time-dependent scattering patterns to obtain the phase diagram of the system and the kinetics of the colloidal and SL phases as a function of varying quench conditions. The extracted phase diagram is consistent with particles whose interactions are short in range relative to their diameter. We find the degree of SL order is primarily determined by fast (subsecond) initial nucleation and growth kinetics, while coarsening at later times depends nonmonotonically on the driving force for self-assembly. We validate these results by direct comparison with simulations and use them to suggest dynamic design principles to optimize the crystallinity within a finite time window. The combination of this measurement methodology, quantitative analysis, and simulation should be generalizable to elucidate and better control the microscopic self-assembly pathways of a wide range of bottom-up assembled systems and architectures.

A series of lanthanide tetrakis-trifluoroacetates {(detaH2)2[La2(tfa)8]2(CH3CN)5(H2O)2}n and (detaH2)n[Ln(tfa)4]2n (Ln = Pr–Eu), mixed-ligand complexes [La(tfa)3(CH3CN)(H2O)]n, [Gd(tfa)3(deta)2](iPrOH) and [Yb(tfa)2(deta)2](tfa), as well as detaH2(tfa)2 were isolated and characterized. All lanthanide tetrakis-trifluoroacetates contain two types of 1D anionic chains [Ln(tfa)4]nn− and cavities occupied by detaH22+ cations and solvating H2O and CH3CN molecules. The thermal behavior of (detaH2)n[Ln(tfa)4]2n in air is investigated by TGA, in situ VT-PXRD and total X-ray scattering with PDF analysis, and the formation of metal fluorides occurs upon heating to 300 °C. The application of solution with lanthanide trifluoroacetates and diethylenetriamine (deta) as precursors for chemical deposition of β-NaGdF4:Er,Yb,Nd thin films is reported. The deposited β-NaGdF4:Er,Yb,Nd thin film demonstrates up-conversion luminescence under 980 and 808 nm laser excitation. [ABSTRACT FROM AUTHOR]

All-solid-state batteries are typically manufactured under high pressure to decrease the resistance of the solid interface. However, until now, there has been a lack of research concerning changes in the structure of solid electrolytes owing to pressurization. Our study addresses this gap by exploring the structural modifications of the sulfide solid electrolyte Li3PS4 under high-pressure conditions. We observed a tendency for PS4 molecules to converge upon each other in both β-Li3PS4 and g-Li3PS4 crystals when subjected to a pressure of 100 MPa. In g-Li3PS4, X-ray scattering and pair distribution function analyses following pressure application and subsequent return to ambient conditions remained consistent with pre-compression measurements. Conversely, in β-Li3PS4 crystals, post-pressure X-ray scattering differed from pre-compression measurements, suggesting pressure-induced atomic rearrangement within the crystal lattice. This underscores the importance of accounting for pressure-induced structural changes, especially in computational simulation studies where crystal structures are often assumed to remain static pre- and post-pressurization. Our findings demonstrate that under high pressure, the crystal structure of Li3PS4 slightly changes by approximately 1~2%, rendering it a viable candidate for utilization as a solid electrolyte in all-solid-state batteries. [ABSTRACT FROM AUTHOR]

Time-resolved studies are crucial for capturing the dynamic evolution of triglyceride structures during crystallization, providing insights into the self-assembly of diverse triglyceride structures across various length scales. While previous research has characterized triglyceride's polymorphisms and long spacings using wide-angle and small-angle X-ray techniques, time-resolved studies on the mesoscale of triglycerides have been limited, particularly in the study of crystalline nanoplatelets (CNPs) and their aggregates. This study pioneers the application of ultra-small-angle X-ray scattering (USAXS) for time-resolved analysis of commercial sources of saturated monoacid triglycerides. The methodology presented here integrates real-time synchrotron X-ray scattering (XRS) with differential scanning calorimetry (DSC), phase contrast microscopy (PCM), and cryo-scanning electron microscopy (Cryo-SEM) to investigate the crystallization behavior of a 30% dilution of palm stearin (PS) in high oleic sunflower oil (HOSO) and a 30% dilution of fully hydrogenated rapeseed oil (FHRO) in HOSO. Covering several orders of magnitude, this comprehensive multiscale approach enhances our kinetic understanding of triglyceride structural transformations. Both systems followed a polymorphic transition from α to β, with a transition from 2L(α) to 2L(β) lamellar stacking configuration. Our results suggest that structural evolutions in non-pure triglyceride systems advance gradually over extended timescales post-crystallization. While lamellae and CNP thicknesses decreased with the polymorphic transition, CNP size and aggregation changed in four distinct phases. We believe that the methodology presented here will greatly improve our understanding of the self-assembly of lipids, getting us closer to bottom-up optimization of triglyceride-based formulations in food. [ABSTRACT FROM AUTHOR]

A spatially modulated superconducting state, known as pair density wave (PDW), is a tantalizing state of matter with unique properties. Recent scanning tunneling microscopy (STM) studies revealed that spin-triplet superconductor UTe2 hosts an unprecedented spin-triplet, multi-component PDW whose three wavevectors are indistinguishable from a preceding charge-density wave (CDW) order that survives to temperatures well above the superconducting critical temperature, Tc. Whether the PDW is the mother or a subordinate order remains unsettled. Here, based on a systematic search for bulk charge order above Tc using resonant elastic X-ray scattering (REXS), we show that the structure factor of charge order previously identified by STM is absent in the bulk within the sensitivity of REXS. Our results invite two scenarios: either the density-wave orders condense simultaneously at Tc in the bulk, in which case PDW order is likely the mother phase, or the charge modulations are restricted to the surface. Surface-sensitive scanning tunneling microscopy (STM) has previously found a charge density wave (CDW) up to 10 K in the normal state of the heavy-fermion superconductor UTe2. Here, using resonant elastic X-ray scattering (REXS) above the superconducting transition, the authors find no evidence for a bulk CDW, suggesting the normal state CDW observed by STM is a surface effect. [ABSTRACT FROM AUTHOR]

Tin chloride pentahydrate (SnCl ${_{{4}}} \cdot 5$ H2O) is used as the dopant precursor to form the n-type $\alpha $ -Ga2O3 in this study. The X-ray diffraction (XRD) and high-resolution transmission electron microscope (HR-TEM) confirm that the single-crystalline $\alpha $ -Ga2O3:SnCl ${_{{4}}} \cdot 5$ H2O epi-layer was grown on the r-plane sapphire substrate using mist chemical vapor deposition (mist-CVD). When the Sn doping atomic concentrations are the same, the electron concentration of $\alpha $ -Ga2O3:SnCl ${_{{4}}} \cdot 5$ H2O is higher than that of $\alpha $ -Ga2O3:SnCl ${_{{2}}} \cdot 2$ H2O. The lower thermal decomposition temperature and lower residues of $\alpha $ -Ga2O3:SnCl ${_{{4}}} \cdot 5$ H2O are confirmed in thermogravimetric (TGA) analysis. Sn $3d_{5/2}$ binding energy spectra observed by X-ray photoelectron spectroscopy (XPS) show that SnCl ${_{{4}}} \cdot 5$ H2O provides more $Sn^{4+}$ than SnCl ${_{{2}}} \cdot 2$ H2O. The specific contact resistivity of $\alpha $ -Ga2O3:SnCl ${_{{4}}} \cdot 5$ H2O reaches $1.62\times 10{^{-}5 }~\Omega $ -cm2 with $10^{20}$ cm $^{-}3 $ Sn doping concentration. Moreover, the power figure-of-merit (PFoM) of $\alpha $ -Ga2O3:SnCl ${_{{4}}} \cdot 5$ H2O-based lateral Schottky barrier diode (SBD) is 0.356 GW/cm2 which is comparable to $\beta $ -Ga2O3-based SBD. [ABSTRACT FROM AUTHOR]

The crystallization behavior of silica-filled polydimethylsiloxane (PDMS) was investigated in detail by 1H solid-state nuclear magnetic resonance (1H SS-NMR) in combination with synchrotron radiation wide-angle X-ray scattering (WAXS), and temperature-modulated differential scanning calorimetry (TMDSC) techniques. For neat PDMS, no apparent difference is observed for the crystallinity characterized by 1H SS-NMR and WAXS at low-temperature regions. However, upon filler addition, a 15%–35% lower difference in crystallinity is observed measured by 1H SS-NMR compared to WAXS. The origin of such mismatch was explored through multi-component structural, dynamics, and chain-order analysis of PDMS samples with different filler fractions. The 1D integrated WAXS results of PDMS with different filler fractions at different temperatures show that the packing structure as well as crystal size basically remain unchanged, but as the filler fraction increases from 0 phr to 60 phr, the rigid component's dynamics order parameter Sr obtained by 1H SS-NMR decreases from 0.70 to 0.55. The filler fraction-dependent crystallinity calculated based on Sr was compared with experimental values, revealing a behavior of decreasing order in the crystalline region. Combining with the results of accelerated chain dynamics in crystalline region as reflected by T2 values, the molecular origin is attributed to the formation of CONDIS crystals, whose conformational order is lost but the position and orientation orders are kept. Such hypothesis is further supported by the TMDSC results, where, as the filler fraction increases from 0 phr to 60 phr, the melting range widens from 8.77 K to 14.56 K, representing a growth of 166%. In addition to previous reports related to the condition for forming CONDIS mesophase, i.e., temperature, pressure, and stretching, the nano-sized filler could also introduce the local conformational disorder for chain packing. [ABSTRACT FROM AUTHOR]

The biosynthesis of bacterial cellulose (BC) is significantly influenced by the type of carbon source available in the growth medium, which in turn dictates the material's final properties. This study systematically investigates the effects of five carbon sources—raffinose (C18H32O16), sucrose (C12H22O11), glucose (C6H12O6), arabinose (C5H10O5), and glycerol (C3H8O3)—on BC production by Komagataeibacter hansenii. The varying molecular weights and structural characteristics of these carbon sources provide a framework for examining their influence on BC yield, fiber morphology, and network properties. BC production was monitored through daily measurements of optical density and pH levels in the fermentation media from day 1 to day 14, providing valuable insights into bacterial growth kinetics and cellulose synthesis rates. Scanning electron microscopy (SEM) was used to elucidate fibril diameter and pore size distribution. Wide-angle X-ray scattering (WAXS) provided a detailed assessment of crystallinity. Selected BC pellicles were further processed via freeze-drying to produce a foam-like material that maximally preserves the natural three-dimensional structure of BC, facilitating the incorporation and release of lidocaine hydrochloride (5%), a widely used local anesthetic. The lidocaine-loaded BC foams exhibited a sustained and controlled release profile over 14 days in simulated body fluid, highlighting the importance of the role of carbon source selection in shaping the BC network architecture and its impact on drug release profile. These results highlight the versatility and sustainability of BC as a platform for wound healing and drug delivery applications. The tunable properties of BC networks provide opportunities for optimizing therapeutic delivery and improving wound care outcomes, positioning BC as an effective material for enhanced wound management strategies. [ABSTRACT FROM AUTHOR]

Xuan paper is a classic Chinese handmade paper with long history and has been listed as a national intangible cultural heritage since 2009, which is mainly composed of wingceltis (Pteroceltis tatarinowii) phloem fibers and straw fibers. Due to the unique properties of wingceltis phloem fibers, Xuan paper is spotless, flexible, stable, and durable, and is widely used by calligraphers, painters, or museums for restoration. Uncovering the variation of phloem fiber properties throughout the traditional pulping process is essential for a comprehensive understanding of the special performance of Xuan paper. In this study, chemical, structural, and mechanical characterization was conducted on the raw bark (phloem fiber), treated phloem fiber, and pulp fiber at different steps of the traditional pulping process for making Xuan paper. The compositional and morphological analysis revealed the effective removal of the matrix polymers, while the phloem fiber almost retained the original fiber structure during the traditional process. Wide-angle X-ray scattering results indicated that the relative crystallinity of cellulose increased and crystals expanded after the lime cooking and exposure to sun and rain. Compared to the raw phloem fibers, the ultimate stress and tensile stiffness of pulp fibers decreased by 24.35% and 9.79%, respectively. However, the fracture strain and fracture toughness of pulp fibers showed a drastic promotion, which might be attributed to the energy dissipation caused by the cell wall structure, the breaking and reforming of hydrogen bonds, and the slipping and rearrangement of cellulose microfibrils. [ABSTRACT FROM AUTHOR]

Research of infinite-layer nickelates has unveiled a broken translation symmetry, which has sparked significant interest in its root, its relationship to superconductivity, and its comparison to charge order in cuprates. In this study, resonant x-ray scattering measurements were performed on thin films of infinite-layer PrNiO2+ δ . The results show significant differences in the superlattice reflection at the Ni L 3 absorption edge compared to that at the Pr M 5 resonance in their dependence on energy, temperature, and local symmetry. These differences point to two distinct charge orders, although they share the same in-plane wavevectors. It is suggested that these dissimilarities could be linked to the excess oxygen dopants, given that the resonant reflections were observed in an incompletely reduced PrNiO2+ δ film. Furthermore, azimuthal analysis indicates that the oxygen ligands likely play a crucial role in the charge modulation revealed at the Ni L 3 resonance. [ABSTRACT FROM AUTHOR]

The present study explores the application of X-ray scattering, using synchrotron radiation, to assess the diffusive transport of nanomedicines in tumor on a chip devices fabricated by 3D stereolithography using a resin with high optical and X-ray transmittance. Unlike conventional methods that require fluorescent labeling of nanoparticles, potentially altering their in vitro and in vivo behavior, this approach enables the investigation of the transport properties for unlabeled nanoparticles. In particular, the results presented confirm the influence of the porosity of the extracellular matrix-like microenvironment, specifically Matrigel, on the diffusive transport of oligonucleotide-functionalized gold nanoparticles. The analysis of the scattering patterns allows to create 2D maps showing the nanoparticle distribution with high spatial resolution. The proposed approach demonstrates the potential for studying other factors involved in nanoparticle diffusion processes. By implementing X-ray scattering to track unmodified nanomedicines within extracellular matrix-like microenvironments, increasingly accurate models for evaluating and predicting therapeutics transport behaviors can be developed. [ABSTRACT FROM AUTHOR]

Resonant inelastic X-ray scattering (RIXS) has played a pivotal role in advancing our understanding of spin-orbit physics in 5d transition metal materials. The progress in RIXS techniques has closely paralleled improvements in energy resolution, which have enabled the study of very low-lying excitations and led to the discovery of numerous new phenomena with significant scientific and technological implications. The multi-bend achromat (MBA) lattice upgrade of third-generation synchrotron sources, such as the Advanced Photon Source (APS), heralds a transformative era by introducing enhancements in brilliance and emittance. These advancements provide an opportunity to push the boundaries of RIXS techniques, meeting the challenges at the research frontiers of material science. This article aims to highlight key instrumental and technical advancements that enable the achievement of meV resolution in RIXS and discuss the impact of such high-resolution RIXS on exploring spin-orbit physics in 5d transition metal materials. [ABSTRACT FROM AUTHOR]

The spontaneous polarisation of the SmCP phase is over two orders of magnitude larger than that found in conventional ferroelectric SmC phase of chiral materials used in some LCD devices. Fully atomistic molecular dynamics simulations faithfully and spontaneously reproduce the proposed structure and associated bulk properties; comparison of experimental and simulated X‐ray scattering patterns shows excellent agreement. The materials disclosed here have significantly smaller dipole moments than typical polar liquid crystals such as RM734 which suggests the role of molecular electrical polarity in generating polar order is perhaps overstated, a view supported by consideration of other molecular systems. [ABSTRACT FROM AUTHOR]

A characteristic feature of cellulose is crystal polymorphism. Among the cellulose allomorphs, cellulose IVII has been the most time-consuming and energy-intensive one to prepare from native cellulose with a cellulose I structure. In this work, we report a facile preparation method of cellulose IVII by regeneration from an ionic liquid (IL) solution. Although regeneration from arbitrary IL solutions is known to produce only cellulose II and amorphous cellulose, we found that appropriate selections of regeneration temperature (373 K), IL structure (dimethylphosphate anion paired with imidazolium cation), and cellulose concentration (5 mol%) induced the formation of cellulose IVII. With the optimal conditions, cellulose IV with crystallinity of 31% was obtained without contamination of other cellulose allomorphs. Wide angle X-ray scattering and 13C solid-state NMR measurements on cellulose/IL mixtures demonstrated that the cations and anions were rather ordered and the gt conformer of cellulose was preferred at a high temperature, which would be relevant for the formation of cellulose IVII. [ABSTRACT FROM AUTHOR]

Although the LiCoO2 (LCO) cathode material has been widely used in commercial lithium ion batteries (LIB) and shows high stability, LIB's improvements have several challenges that still need to be overcome. In this paper, we have studied the in-operando structural properties of LCO within battery cells using Bragg Coherent X-ray Diffraction Imaging to identify ways to optimise the LCO batteries' cycling. We have successfully reconstructed the X-ray scattering phase variation (a fingerprint of atomic displacement) within a ≈ (1.6 × 1.4 × 1.3) μm3 LCO nanocrystal across a charge/discharge cycle. Reconstructions indicate strained domains forming, expanding, and fragmenting near the surface of the nanocrystal during charging, with a determined maximum relative lattice displacements of 0.467 Å. While discharging, all domains replicate in reverse the effects observed from the charging states, but with a lower maximum relative lattice displacements of 0.226 Å. These findings show the inefficiency-increasing domain dynamics within LCO lattices during cycling. Although lithium cobalt(III) oxide (LCO) is a widely used and highly stable lithium-ion battery material, several challenges still need to be overcome. Here, the authors use in-operando Bragg Coherent X-ray Diffraction Imaging to visualize the structural properties of LCO in battery cells and identify inefficiency-increasing domain dynamics during cycling. [ABSTRACT FROM AUTHOR]

Colloidal lead halide perovskite nanocrystals have potential for lighting applications due to their optical properties. Precise control of the nanocrystal dimensions and composition is a prerequisite for establishing practical applications. However, the rapid nature of their synthesis precludes a detailed understanding of the synthetic pathways, thereby limiting the optimisation. Here, we deduce the formation mechanisms of anisotropic lead halide perovskite nanocrystals, 1D nanorods and 2D nanoplatelets, by combining in situ X-ray scattering and photoluminescence spectroscopy. In both cases, emissive prolate nanoclusters form when the two precursor solutions are mixed. The ensuing antisolvent addition induces the divergent anisotropy: The intermediate nanoclusters are driven into a dense hexagonal mesophase, fusing to form nanorods. Contrastingly, nanoplatelets grow freely dispersed from dissolving nanoclusters, stacking subsequently in lamellar superstructures. Shape and size control of the nanocrystals are determined primarily by the antisolvent's dipole moment and Hansen hydrogen bonding parameter. Exploiting the interplay of antisolvent and organic ligands could enable more complex nanocrystal geometries in the future. Lead halide perovskite nanocrystals show bright and colour-pure emission in the visible range, which can be tuned by nanocrystal size and composition. Here authors present the formation mechanisms of anisotropic lead halide perovskite nanocrystals, 1D nanorods and 2D nanoplatelets, by combining in situ X-ray scattering and photoluminescence spectroscopy. [ABSTRACT FROM AUTHOR]

Resonant inelastic X-ray scattering (RIXS) has played a pivotal role in advancing our understanding of spin-orbit physics in 5d transition metal materials. The progress in RIXS techniques has closely paralleled improvements in energy resolution, which have enabled the study of very low-lying excitations and led to the discovery of numerous new phenomena with significant scientific and technological implications. The multi-bend achromat (MBA) lattice upgrade of third-generation synchrotron sources, such as the Advanced Photon Source (APS), heralds a transformative era by introducing enhancements in brilliance and emittance. These advancements provide an opportunity to push the boundaries of RIXS techniques, meeting the challenges at the research frontiers of material science. This article aims to highlight key instrumental and technical advancements that enable the achievement of meV resolution in RIXS and discuss the impact of such high-resolution RIXS on exploring spin-orbit physics in 5d transition metal materials. [ABSTRACT FROM AUTHOR]

[Display omitted] Organohydrogel emulsions display unique rheological properties and contain hydrophilic and lipophilic domains highly desirable for the loading of active compounds. They find utility in various applications from food to pharmaceuticals and cosmetic products. The current systems have limited applications due to complex expensive formulation and/or processing difficulties in scale-up. To solve these issues, a simple emulsification process coupled with unique compounds are required. Here, we report an organohydrogel emulsion based only on a low concentration of 12-hydroxystearic acid acting as a gelling agent for both oil and water phases but also as a surfactant. The emulsification process is based on in-situ surfactant transfer. We characterize the emulsification process occurring at the nanoscale by using tensiometry experiments. The emulsion structure was determined by coupling Small Angle X-ray and neutron scattering, and confocal Raman microscopy. We demonstrate that the stability and unique rheological properties of these emulsions come from the presence of self-assembled crystalline structures of 12-hydroxystearic acid in both liquid phases. The emulsion properties can be tuned by varying the emulsion composition over a wide range. These gelled emulsions are prepared using a low energy method offering easy scale-up at an industrial level. [ABSTRACT FROM AUTHOR]

Calcium (Ca2+) signaling is fundamental to cellular processes in both eukaryotic and prokaryotic organisms. While the mechanisms underlying eukaryotic Ca2+ transport are well documented, an understanding of prokaryotic transport remains nascent. LMCA1, a Ca2+ adenosine triphosphatase (ATPase) from Listeria monocytogenes, has emerged as a prototype for elucidating structure and dynamics in prokaryotic Ca2+ transport. Here, we used a multidisciplinary approach integrating kinetics, structure, and dynamics to unravel the intricacies of LMCA1 function. A cryo-electron microscopy (cryo-EM) structure of a Ca2+-bound E1 state showed ion coordination by Asp720, Asn716, and Glu292. Time-resolved x-ray solution scattering experiments identified phosphorylation as the rate-determining step. A cryo-EM E2P state structure exhibited remarkable similarities to a SERCA1a E2-P* state, which highlights the essential role of the unique P-A domain interface in enhancing dephosphorylation rates and reconciles earlier proposed mechanisms. Our study underscores the distinctiveness between eukaryotic and prokaryotic Ca2+ ATPase transport systems and positions LMCA1 as a promising drug target for developing antimicrobial strategies. [ABSTRACT FROM AUTHOR]

The results of investigation of DNA-protein complexes by two independent structural methods, namely, molecular dynamics (MD) and small-angle X-ray scattering (SAXS), were compared. Molecular dynamics is a computational method enabling the visualization of the behavior of macromolecules in real media, which is based on the laws of physics, but it is limited by numerous simplifications. Small-angle X-ray scattering is an X-ray method, which allows the reconstruction of the three-dimensional structure of a system in solution from a one-dimensional small-angle scattering profile, but it faces the problem of ambiguity in solving inverse problems. The use of structural characteristics of the complexes determined by SAXS for the validation of 3D structural models generated by MD simulations made it possible to significantly reduce the ambivalence of theoretical predictions and demonstrated the efficiency of a combination of MD simulations and SAXS for solving problems of structural biology. [ABSTRACT FROM AUTHOR]

"MightyLev," a new multi-emitter ultrasonic acoustic levitation device capable of extremely stable levitation of materials of density up to at least 11.3 g cm−3, is described. The exceptional stability of medium- to high-density samples levitated in MightyLev makes the device highly suitable for chemical and structural analysis using micro-focused spectroscopic and x-ray scattering techniques. In combination with mid-infrared laser heating, MightyLev is capable of levitating metallic and oxide materials during high-temperature cycling and melting above 1500 K. Instabilities in particle confinement during heating were investigated by directly visualizing the acoustic field using schlieren imaging. The results reveal jets of hot-air directed along the anti-nodes of the acoustic field. The reaction force on the sample from the jet, coupled with the restoring force of the acoustic trap, generates a parametric lateral oscillation of the sample. This result provides valuable insight for future optimization and wider application of acoustic levitation for high-temperature containerless material processing. [ABSTRACT FROM AUTHOR]

Poly(p-dioxanone) (PPDO) is crystallized with amorphous poly(p-vinyl phenol) (PVPh) and tannic acid (TA) as co-diluents to regulate and induce dendritic-ringed PPDO spherulites, with spoke- or sector-bands, aiming for convenience of analyses on interior lamellar assembly. Morphologies and interior lamellar arrangement leading to the peculiar rings on individual dendrites are evaluated by using polarized-light microscopy (PLM) and scanning electron microscope (SEM). Combinatory microbeam small-/wide-angle X-ray scattering (SAXS/WAXS) analyses further confirm the unique assembly patterns in periodic cycles. Alternate gratings are packed with periodic ridges composed of feather-like branches and the valley is featured with some embossed textures. The periodic gratings in the ringed spokes resemble those in nature's structured coloration and are proven to display light-interference iridescence. [ABSTRACT FROM AUTHOR]

X‐ray scattering has become a major tool in the structural characterization of nanoscale materials. Thanks to the widely available experimental and computational atomic models, coordinate‐based X‐ray scattering simulation has played a crucial role in data interpretation in the past two decades. However, simulation of real‐space pair distance distribution functions (PDDFs) from small‐ and wide‐angle X‐ray scattering, SAXS/WAXS, has been relatively less exploited. This study presents a comparison of PDDF simulation methods, which are applied to molecular structures that range in size from β‐cyclodextrin [1 kDa molecular weight (MW), 66 non‐hydrogen atoms] to the satellite tobacco mosaic virus capsid (1.1 MDa MW, 81960 non‐hydrogen atoms). The results demonstrate the power of interpretation of experimental SAXS/WAXS from the real‐space view, particularly by providing a more intuitive method for understanding of partial structure contributions. Furthermore, the computational efficiency of PDDF simulation algorithms makes them attractive as approaches for the analysis of large nanoscale materials and biological assemblies. The simulation methods demonstrated in this article have been implemented in stand‐alone software, SolX 3.0, which is available to download from https://12idb.xray.aps.anl.gov/solx.html. [ABSTRACT FROM AUTHOR]

Understanding the structure–property relationship in electrocatalysts under working conditions is crucial for the rational design of novel and improved catalytic materials. This paper presents the Aarhus University reactor for electrochemical studies using X‐rays (AUREX) operando electrocatalytic flow cell, designed as an easy‐to‐use versatile setup with a minimal background contribution and a uniform flow field to limit concentration polarization and handle gas formation. The cell has been employed to measure operando total scattering, diffraction and absorption spectroscopy as well as simultaneous combinations thereof on a commercial silver electrocatalyst for proof of concept. This combination of operando techniques allows for monitoring of the short‐, medium‐ and long‐range structure under working conditions, including an applied potential, liquid electrolyte and local reaction environment. The structural transformations of the Ag electrocatalyst are monitored with non‐negative matrix factorization, linear combination analysis, the Pearson correlation coefficient matrix, and refinements in both real and reciprocal space. Upon application of an oxidative potential in an Ar‐saturated aqueous 0.1 M KHCO3/K2CO3 electrolyte, the face‐centered cubic (f.c.c.) Ag gradually transforms first to a trigonal Ag2CO3 phase, followed by the formation of a monoclinic Ag2CO3 phase. A reducing potential immediately reverts the structure to the Ag (f.c.c.) phase. Following the electrochemical‐reaction‐induced phase transitions is of fundamental interest and necessary for understanding and improving the stability of electrocatalysts, and the operando cell proves a versatile setup for probing this. In addition, it is demonstrated that, when studying electrochemical reactions, a high energy or short exposure time is needed to circumvent beam‐induced effects. [ABSTRACT FROM AUTHOR]

Additive Manufacturing (AM) has revolutionised the production of custom-shaped samples through direct manufacturing from digital design models. As the internal structural integrity of these printed samples is of critical importance in diverse applications, X-ray radiography and X-ray Computer Tomography (X-CT) have emerged as widely used non-destructive imaging methods for quality control of AM samples. Unfortunately, beam hardening and X-ray scatter often degrade the quality of X-CT images, posing a significant challenge for X-ray based inspection. In addressing X-ray scatter, most of the methodologies assume fixed scanning geometries or stationary/known object characteristics, limiting their practicality in dynamic industrial scenarios where these may change over time. Simulation-based methods have been proposed that estimate and suppress scatter by accurately simulating the forward projection process. Yet, these methods assume the availability of X-CT reconstruction for simulation, thereby requiring a large number of projections (and hence scan time) for faithful X-CT reconstruction. In this work, we propose a simulation-based scatter compensation method (PACS) that eliminates the need for a prior X-CT scan. By employing few projections and nominal surface meshes of the scanned objects, the actual pose of the objects and their superficial deviation (e.g., due to printing) are estimated and used during X-ray simulations. Furthermore, as the pipeline is inherently coupled with a mesh projector, analysis of projective residuals facilitates the inspection for deformities or defects within the scanned object. To demonstrate the versatility of PACS for mitigating scatter, experiments across various inspection scenarios are conducted, and the outcomes are compared with those of a well-established scatter compensation technique. The results consistently show a higher Signal-to-Noise Ratio and Contrast-to-Noise Ratio of pore-defects, as well as lower residual errors in all examined cases. • Adaptable X-ray scatter compensation specifically tailored for inspection of Additive Manufacturing samples. • Simulation-based approach that eliminates the need for prior X-ray tomographic reconstruction. • Acceleration patterns enhance the speed of Monte Carlo simulations. • By integrating a mesh projector, direct defect detection is enabled through residual analysis. [ABSTRACT FROM AUTHOR]

Accreting stellar-mass black holes represent unique laboratories for studying matter and radiation under the influence of extreme gravity. They are highly variable sources going through different accretion states, showing various components in their X-ray spectra from the thermal emission of the accretion disc dominating in the soft state to the up-scattered Comptonisation component from an X-ray corona in the hard state. X-ray polarisation measurements are particularly sensitive to the geometry of the X-ray scatterings and can thus constrain the orientation and relative positions of the innermost components of these systems. The IXPE mission has observed about a dozen stellar-mass black holes with masses up to 20 solar masses in X-ray binaries with different orientations and in various accretion states. The low-inclination sources in soft states have shown a low fraction of polarisation. On the other hand, several sources in soft and hard states have revealed X-ray polarisation higher than expected, which poses significant challenges for theoretical interpretation, with 4U 1630–47 being one of the most puzzling sources. IXPE has measured the spin of three black holes via the measurement of their polarisation properties in the soft emission state. In each of the three cases, the new results agree with the constraints from the spectral observations. The polarisation observations of the black hole X-ray transient Swift J1727.8–1613 across its entire outburst has revealed that the soft-state polarisation is much weaker than the hard-state polarisation. Remarkably, the observations furthermore show that the polarisation of the bright hard state and that of the 100 times less luminous dim hard state are identical within the accuracy of the measurement. For sources with a radio jet, the electric field polarisation tends to align with the radio jet, indicating the equatorial geometry of the X-ray corona, e.g., in the case of Cyg X–1. In the unique case of Cyg X–3, where the polarisation is perpendicular to the radio jet, the IXPE observations reveal the presence and geometry of obscuring material hiding this object from our direct view. The polarisation measurements acquired by the IXPE mission during its first 2.5 years have provided unprecedented insights into the geometry and physical processes of accreting stellar-mass black holes, challenging existing theoretical models and offering new avenues for understanding these extreme systems. [ABSTRACT FROM AUTHOR]

Oleogelation is an alternative oil structuring route to formulate (semi-)solid fats with a reduced amount of saturated fats. Monoglycerides have been identified as effective gelators; however, their application potential can be limited due to challenges regarding mechanical strength and long-term stability. Therefore, the formulation of hybrid fat blends is a promising way to improve the functionality of oleogels. This research focuses on the interaction between mono- and triglycerides (MAGs and TAGs) in hybrid oleogels. A total gelator concentration of 10% (w/w) with changing MAGs–TAGs ratios (increase by 25% on a molar basis; M0-T100, M25-T75, M50-T50, M75-T25, M100-T0) was used. First, the oleogels were produced without shear to unravel the crystallization behavior (DSC, SAXS, WAXS). Next, the oleogels were crystallized with shear to assess the interactions between MAGs and TAGs on macroscale properties (rigidity, oil binding capacity) during storage of 1 day, 1 week, and 4 weeks. A clear distinction could be made between the MAG crystals and TAG crystals in the blends M50-T50 and M75-T25 based on WAXS, SAXS, and phase contrast microscopy. This indicates that both gelators crystallize separately. During the follow-up study of the dynamically produced samples, a synergistic effect was found for Dy-M50-T50 and Dy-M75-T25; however, it was not maintained upon storage. The initial rigidity of 2.4 × 104 Pa and 2.0 × 104 Pa decreased to 1.5 × 104 Pa and 1.0 × 104 Pa for Dy-M50-T50 and Dy-M75-T25, respectively. [ABSTRACT FROM AUTHOR]

Structural studies using x-ray scattering methods for investigating molecules in solution are shifting focus toward describing the role and effects of the surrounding solvent. However, forward models based on molecular dynamics (MD) simulations to simulate structure factors and x-ray scattering from interatomic distributions such as radial distribution functions (RDFs) face limitations imposed by simulations, particularly at low values of the scattering vector q. In this work, we show how the value of the structure factor at q = 0 calculated from RDFs sampled from finite MD simulations is effectively dependent on the size of the simulation cell. To eliminate this error, we derive a new scheme to renormalize the sampled RDFs based on a model of the excluded volume of the particle-pairs they were sampled from, to emulate sampling from an infinite system. We compare this new correction method to two previous RDF-correction methods, developed for Kirkwood–Buff theory applications. We present a quantitative test to assess the reliability of the simulated low-q scattering signal and show that our RDF-correction successfully recovers the correct q = 0 limit for neat water. We investigate the effect of MD-sampling time on the RDF-corrections, before advancing to a molecular example system, comprised of a transition metal complex solvated in a series of water cells with varying densities. We show that our correction recovers the correct q = 0 behavior for all densities. Furthermore, we employ a simple continuum scattering model to dissect the total scattering signal from the solvent–solvent structural correlations in a solute–solvent model system to find two distinct contributions: a non-local density-contribution from the finite, fixed cell size in NVT simulations, and a local contribution from the solvent shell. We show how the second contribution can be approximated without also including the finite-size contribution. Finally, we provide a "best-practices"-checklist for experimentalists planning to incorporate explicit solvation MD simulations in future work, offering guidance for improving the accuracy and reliability of structural studies using x-ray scattering methods in solution. [ABSTRACT FROM AUTHOR]

We investigate the role of Compton ionization in ultrafast non-resonant x-ray scattering using a molecular model system, which includes the ionization continuum via an orthonormalized plane wave ansatz. Elastic and inelastic components of the scattering signal, as well as coherent-mixed scattering that arises from electron dynamics, are calculated. By virtue of a near-quantitative distinction between scattering related to electronic transitions into bound and continuum states, we demonstrate how Compton ionization contributes to the coherent-mixed component. Analogous to inelastic scattering, the contribution to the coherent-mixed signal is significant and particularly manifests at intermediate and high-momentum transfers. Strikingly, for molecules with inversion symmetry, the exclusion of bound or continuum transitions may lead to the prediction of spurious coherent-mixed signals. We conclude that qualitative and quantitative accuracies of predicted scattering signals on detectors without energy resolution require that elements of the two-electron density operator are used. This approach inherently accounts for all accessible electronic transitions, including ionization. [ABSTRACT FROM AUTHOR]

[Display omitted] Acoustic levitation is a suitable approach for studying processes occurring at the gas–liquid interfaces, as it allows its investigation in a contact-free manner while providing control over the gas phase. Here, we hypothesize that phase transitions induced by a CO 2 rich atmosphere can be examined, at different length scales, in a contact-free manner. A system consisting of 12-hydroxysteric acid (HSA) soaps mixed with different ratios of monoethanolamine (MEA) and choline hydroxide, was prepared. Microliter droplets of the samples were acoustically levitated and monitored with a camera, while exposed to CO 2 to modify the pH through diffusion at the air–liquid interface and inside the droplet. The phase transition and water mobility in the levitated droplets were evaluated through X-ray scattering (SAXS/WAXS) and magnetic resonance studies, in real-time. Finally, the droplets were collected and examined under the microscope. The introduction of CO 2 gas induced a phase transition from micelles to multi-lamellar tubes, resulting in a gel-like behavior both in the bulk and at the interface. The high stability of the acoustic levitator allowed the investigation of this dynamic phenomenon, in real-time, in a contact-free environment. This study showcases the suitability of acoustic levitation as a tool to investigate complex chemical processes at interfaces. [ABSTRACT FROM AUTHOR]